US20230268546A1 - Battery cell - Google Patents
Battery cell Download PDFInfo
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- US20230268546A1 US20230268546A1 US18/169,832 US202318169832A US2023268546A1 US 20230268546 A1 US20230268546 A1 US 20230268546A1 US 202318169832 A US202318169832 A US 202318169832A US 2023268546 A1 US2023268546 A1 US 2023268546A1
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- negative electrode
- layer
- active material
- electrode active
- battery cell
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- 239000007773 negative electrode material Substances 0.000 claims abstract description 46
- 239000003792 electrolyte Substances 0.000 claims abstract description 42
- 239000007784 solid electrolyte Substances 0.000 claims abstract description 27
- 229910052744 lithium Inorganic materials 0.000 claims abstract description 12
- 210000004027 cell Anatomy 0.000 abstract description 42
- 210000001787 dendrite Anatomy 0.000 abstract description 17
- 230000008021 deposition Effects 0.000 abstract description 7
- 238000000034 method Methods 0.000 description 13
- 239000007774 positive electrode material Substances 0.000 description 11
- 230000000052 comparative effect Effects 0.000 description 8
- 239000000126 substance Substances 0.000 description 8
- 239000013078 crystal Substances 0.000 description 7
- 238000003825 pressing Methods 0.000 description 7
- -1 graphite Chemical class 0.000 description 6
- 239000012752 auxiliary agent Substances 0.000 description 4
- 239000011230 binding agent Substances 0.000 description 4
- 239000007772 electrode material Substances 0.000 description 4
- 239000010935 stainless steel Substances 0.000 description 4
- 229910001220 stainless steel Inorganic materials 0.000 description 4
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 3
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 3
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 3
- 239000008151 electrolyte solution Substances 0.000 description 3
- 238000010030 laminating Methods 0.000 description 3
- 239000011244 liquid electrolyte Substances 0.000 description 3
- 229910001416 lithium ion Inorganic materials 0.000 description 3
- 238000004519 manufacturing process Methods 0.000 description 3
- 229910052751 metal Inorganic materials 0.000 description 3
- 239000002184 metal Substances 0.000 description 3
- 239000002904 solvent Substances 0.000 description 3
- 238000012360 testing method Methods 0.000 description 3
- 229910009511 Li1.5Al0.5Ge1.5(PO4)3 Inorganic materials 0.000 description 2
- 229910003405 Li10GeP2S12 Inorganic materials 0.000 description 2
- 229910011244 Li3xLa2/3-xTiO3 Inorganic materials 0.000 description 2
- 229910011245 Li3xLa2/3−xTiO3 Inorganic materials 0.000 description 2
- 229910002984 Li7La3Zr2O12 Inorganic materials 0.000 description 2
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 description 2
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 2
- 229910052782 aluminium Inorganic materials 0.000 description 2
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 2
- 229910052802 copper Inorganic materials 0.000 description 2
- 239000010949 copper Substances 0.000 description 2
- 238000009826 distribution Methods 0.000 description 2
- 239000011888 foil Substances 0.000 description 2
- 239000010439 graphite Substances 0.000 description 2
- 229910002804 graphite Inorganic materials 0.000 description 2
- KWGKDLIKAYFUFQ-UHFFFAOYSA-M lithium chloride Chemical compound [Li+].[Cl-] KWGKDLIKAYFUFQ-UHFFFAOYSA-M 0.000 description 2
- 239000000463 material Substances 0.000 description 2
- 150000004767 nitrides Chemical class 0.000 description 2
- 230000000452 restraining effect Effects 0.000 description 2
- 239000007787 solid Substances 0.000 description 2
- 239000000758 substrate Substances 0.000 description 2
- 238000003826 uniaxial pressing Methods 0.000 description 2
- 229910005833 GeO4 Inorganic materials 0.000 description 1
- 239000002227 LISICON Substances 0.000 description 1
- 229910000733 Li alloy Inorganic materials 0.000 description 1
- 229910003554 Li(Ni0.25Mn0.75)2O4 Inorganic materials 0.000 description 1
- 229910008026 Li1+x+yAlxTi2-xSiyP3-yO12 Inorganic materials 0.000 description 1
- 229910008043 Li1+x+yAlxTi2−xSiyP3-yO12 Inorganic materials 0.000 description 1
- 229910006188 Li1+x+yAlxTi2−xSiyP3−yO12 Inorganic materials 0.000 description 1
- 229910006210 Li1+xAlxTi2-x(PO4)3 Inorganic materials 0.000 description 1
- 229910006212 Li1+xAlxTi2−x(PO4)3 Inorganic materials 0.000 description 1
- 229910008706 Li2NiMn3O8 Inorganic materials 0.000 description 1
- 229910001216 Li2S Inorganic materials 0.000 description 1
- 229910010848 Li6PS5Cl Inorganic materials 0.000 description 1
- 229910013375 LiC Inorganic materials 0.000 description 1
- 229910001559 LiC4F9SO3 Inorganic materials 0.000 description 1
- 229910000552 LiCF3SO3 Inorganic materials 0.000 description 1
- 229910012735 LiCo1/3Ni1/3Mn1/3O2 Inorganic materials 0.000 description 1
- 229910012808 LiCoMnO4 Inorganic materials 0.000 description 1
- 229910032387 LiCoO2 Inorganic materials 0.000 description 1
- 229910011279 LiCoPO4 Inorganic materials 0.000 description 1
- 229910011638 LiCrO2 Inorganic materials 0.000 description 1
- 229910052493 LiFePO4 Inorganic materials 0.000 description 1
- 229910000668 LiMnPO4 Inorganic materials 0.000 description 1
- 229910013385 LiN(SO2C2F5)2 Inorganic materials 0.000 description 1
- 229910013394 LiN(SO2CF3) Inorganic materials 0.000 description 1
- 229910003005 LiNiO2 Inorganic materials 0.000 description 1
- 229910001290 LiPF6 Inorganic materials 0.000 description 1
- 229910012305 LiPON Inorganic materials 0.000 description 1
- 229910012981 LiVO2 Inorganic materials 0.000 description 1
- 229910002097 Lithium manganese(III,IV) oxide Inorganic materials 0.000 description 1
- 229910014892 LixPOyNz Inorganic materials 0.000 description 1
- 229910019714 Nb2O3 Inorganic materials 0.000 description 1
- 239000004698 Polyethylene Substances 0.000 description 1
- 239000004743 Polypropylene Substances 0.000 description 1
- 229910021131 SiyP3−yO12 Inorganic materials 0.000 description 1
- UCKMPCXJQFINFW-UHFFFAOYSA-N Sulphide Chemical compound [S-2] UCKMPCXJQFINFW-UHFFFAOYSA-N 0.000 description 1
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 1
- 239000000010 aprotic solvent Substances 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 239000003575 carbonaceous material Substances 0.000 description 1
- 150000004649 carbonic acid derivatives Chemical class 0.000 description 1
- 238000005253 cladding Methods 0.000 description 1
- 239000011248 coating agent Substances 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- 238000007796 conventional method Methods 0.000 description 1
- 239000011889 copper foil Substances 0.000 description 1
- 230000003247 decreasing effect Effects 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 238000007606 doctor blade method Methods 0.000 description 1
- 150000002148 esters Chemical class 0.000 description 1
- 150000002170 ethers Chemical class 0.000 description 1
- 150000004820 halides Chemical class 0.000 description 1
- 229910021385 hard carbon Inorganic materials 0.000 description 1
- LHJOPRPDWDXEIY-UHFFFAOYSA-N indium lithium Chemical compound [Li].[In] LHJOPRPDWDXEIY-UHFFFAOYSA-N 0.000 description 1
- 150000002596 lactones Chemical class 0.000 description 1
- 239000001989 lithium alloy Substances 0.000 description 1
- 229910000664 lithium aluminum titanium phosphates (LATP) Inorganic materials 0.000 description 1
- PQXKHYXIUOZZFA-UHFFFAOYSA-M lithium fluoride Inorganic materials [Li+].[F-] PQXKHYXIUOZZFA-UHFFFAOYSA-M 0.000 description 1
- HSZCZNFXUDYRKD-UHFFFAOYSA-M lithium iodide Inorganic materials [Li+].[I-] HSZCZNFXUDYRKD-UHFFFAOYSA-M 0.000 description 1
- IDBFBDSKYCUNPW-UHFFFAOYSA-N lithium nitride Chemical compound [Li]N([Li])[Li] IDBFBDSKYCUNPW-UHFFFAOYSA-N 0.000 description 1
- MHCFAGZWMAWTNR-UHFFFAOYSA-M lithium perchlorate Chemical compound [Li+].[O-]Cl(=O)(=O)=O MHCFAGZWMAWTNR-UHFFFAOYSA-M 0.000 description 1
- 229910001486 lithium perchlorate Inorganic materials 0.000 description 1
- 229910000921 lithium phosphorous sulfides (LPS) Inorganic materials 0.000 description 1
- 229910001496 lithium tetrafluoroborate Inorganic materials 0.000 description 1
- 229910021437 lithium-transition metal oxide Inorganic materials 0.000 description 1
- 229910052976 metal sulfide Inorganic materials 0.000 description 1
- 150000002739 metals Chemical class 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 150000002825 nitriles Chemical class 0.000 description 1
- 239000010450 olivine Substances 0.000 description 1
- 229910052609 olivine Inorganic materials 0.000 description 1
- 239000002245 particle Substances 0.000 description 1
- 229920000573 polyethylene Polymers 0.000 description 1
- 229920001155 polypropylene Polymers 0.000 description 1
- 238000002360 preparation method Methods 0.000 description 1
- 239000002002 slurry Substances 0.000 description 1
- 229910021384 soft carbon Inorganic materials 0.000 description 1
- 229910052596 spinel Inorganic materials 0.000 description 1
- 239000011029 spinel Substances 0.000 description 1
- 150000003457 sulfones Chemical class 0.000 description 1
- 238000012546 transfer Methods 0.000 description 1
- 229910000314 transition metal oxide Inorganic materials 0.000 description 1
- ZNOKGRXACCSDPY-UHFFFAOYSA-N tungsten(VI) oxide Inorganic materials O=[W](=O)=O ZNOKGRXACCSDPY-UHFFFAOYSA-N 0.000 description 1
Images
Classifications
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0561—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of inorganic materials only
- H01M10/0562—Solid materials
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/058—Construction or manufacture
- H01M10/0585—Construction or manufacture of accumulators having only flat construction elements, i.e. flat positive electrodes, flat negative electrodes and flat separators
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/04—Processes of manufacture in general
- H01M4/0402—Methods of deposition of the material
- H01M4/0404—Methods of deposition of the material by coating on electrode collectors
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/134—Electrodes based on metals, Si or alloys
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/139—Processes of manufacture
- H01M4/1395—Processes of manufacture of electrodes based on metals, Si or alloys
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/362—Composites
- H01M4/366—Composites as layered products
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
- H01M4/381—Alkaline or alkaline earth metals elements
- H01M4/382—Lithium
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- H—ELECTRICITY
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- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
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- H01M2004/021—Physical characteristics, e.g. porosity, surface area
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- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
- H01M2004/027—Negative electrodes
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M2300/00—Electrolytes
- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0065—Solid electrolytes
- H01M2300/0068—Solid electrolytes inorganic
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
Definitions
- the present invention relates to battery cells.
- a secondary battery has a structure in which a solid electrolyte (separator) is provided between a positive electrode and a negative electrode and which is filled with a liquid or solid electrolyte (electrolytic solution).
- lithium metals such as lithium metal are used.
- lithium metal is used as a negative electrode active material
- the short circuit may occur when uneven distribution of restraining load occurs.
- Patent Document 1 Japanese Unexamined Patent Application, Publication No. H6-84512
- Patent Document 1 The technique disclosed in Patent Document 1 is capable of suppressing generation of large dendrite crystals by forming fine irregularities on the substrate surface, but when the technique is applied to, for example, a solid-state battery, a strong restraining load is applied to the electrode, so that generation of even relatively small dendrite crystals may affect battery performance. Therefore, under the current state of development, satisfactory cycle characteristics during charge and discharge of the battery cell have not yet been obtained.
- the present invention has been made in view of the above-mentioned circumstances, and it is an object of the present invention to provide a battery cell capable of suppressing deposition of dendrites and improving cycle characteristics.
- a first aspect of the present invention relates to a battery cell having a negative electrode layer, an electrolyte layer, and a positive electrode layer, the negative electrode layer including a negative electrode active material layer that has at least one recess portion and at least one planar portion on a surface of the negative electrode active material layer, the surface being adjacent to the electrolyte layer, the recess portion being a cone or pyramid-shaped recess portion having a slant portion.
- a battery cell capable of suppressing deposition of dendrites and improving cycle characteristics can be provided.
- a second aspect of the present invention relates to the battery cell as described in the first aspect, in which the negative electrode active material layer contains lithium metal.
- the negative electrode active material even when lithium metal which easily produces dendrites is used as the negative electrode active material, occurrence of short circuit can be suppressed, and a battery cell having preferable cycle characteristics can be provided.
- a third aspect of the present invention relates to the battery cell as described in the first or second aspect, in which the electrolyte layer is a solid electrolyte layer including a solid electrolyte.
- the third aspect even in a battery cell having a solid electrolyte layer containing a solid electrolyte as the electrolyte layer, occurrence of short circuit can be suppressed, and a battery cell having preferable cycle characteristics can be provided.
- a fourth aspect of the present invention relates to the battery cell as described in any one of the first to third aspects, in which the at least one recess portion and the at least one planar portion comprise a plurality of recess portions and a plurality of planar portions, respectively, and the plurality of planar portions are formed in a manner that the plurality of recess portions are not in contact with each other.
- the fourth aspect even when a plurality of recess portions is formed in the negative electrode active material layer, no projective portions are formed on a surface of the negative electrode active material layer, the surface being adjacent to the electrolyte layer, and accordingly dendrites can be generated preferentially in the recess portions, which more preferably suppresses occurrence of short circuit of the battery cell.
- FIG. 1 is a cross-sectional view illustrating a configuration of a battery cell according to an embodiment of the present invention
- FIG. 2 is a top view illustrating a part of the negative electrode active material layer according to an embodiment of the present invention.
- FIG. 3 is a graph illustrating results of cycle characteristic tests using the battery cells of the Example and the Comparative Example.
- the battery cell 1 is formed by laminating a negative electrode layer 20 , an electrolyte layer 4 , and a positive electrode layer 30 in this order.
- the battery cell 1 is, for example, a lithium-ion battery cell using lithium ions as a charge transfer medium.
- the battery cell 1 may be a battery cell having a liquid electrolyte layer 4 .
- the battery cell 1 according to the present embodiment is preferably a battery cell having a solid electrolyte layer 4 which is susceptible to the influence of the deposition of dendrites.
- the negative electrode layer 20 is formed, for example, by forming a negative electrode active material layer 22 on a negative electrode current collector 21 .
- the negative electrode current collector 21 is not particularly limited, and a well-known substance can be applied as the negative electrode current collector of a solid secondary battery.
- Examples of the negative electrode current collector 21 include copper, stainless steel, and the like. Copper, stainless steel, and the like are molded into, for example, a foil shape and used.
- the negative electrode active material layer 22 is a layer containing a negative electrode active material as an essential component.
- the negative electrode active material layer 22 may contain a binder, a conductive auxiliary agent, an electrolyte, and the like.
- the binder, the conductive auxiliary agent, the electrolyte, and the like are not particularly limited, and known substances can be used as the electrode material for a secondary battery.
- the negative electrode active material is not particularly limited, and a known substance can be applied as the negative electrode active material for the secondary batteries.
- the configuration of the present embodiment described below can preferably reduce the influence of deposition of dendrites, which is significant when lithium metal is used as the negative electrode active material.
- the negative electrode active material layer 22 preferably contains lithium metal as the negative electrode active material.
- lithium transition metal oxides such as lithium titanate (Li 4 Ti 5 O 12 ); transition metal oxides such as TiO 2 , Nb 2 O 3 , WO 3 , etc.; metal sulfides; metal nitrides; carbon materials such as graphite, soft carbon, hard carbon, etc.; metal indium; lithium alloys; and the like.
- the negative electrode active material layer 22 has a plurality of recess portions 22 a and a plurality of planar portions 22 b on the surface of the negative electrode active material layer 22 , the surface being adjacent to the electrolyte layer 4 .
- a recess portion 22 a is a cone or pyramid-shaped recess portion having a slant portion S. Since the recess portions 22 a are formed in the negative electrode active material layer 22 , the current density varies, and the current density increases in the vicinity of the recess portions 22 a . As a result, since dendrites are preferentially generated at the recess portion 22 a , the risk that the dendrites break through the electrolyte layer 4 and short circuit occurs can be reduced. Thereby, the cycle characteristics of the battery cell 1 can be improved.
- the recess portion 22 a can alleviate unevenness of pressure distribution caused by expansion of the negative electrode layer 20 during charge of the battery cell 1 . Further, since the contact area between the electrolyte layer 4 and the negative electrode active material layer 22 is increased by the recess portion 22 a , resistance is reduced, and thus the output of the battery cell 1 is improved.
- the recess portion 22 a has a shape of cone or pyramid having a slant portion S, a dendrite is likely to be preferentially generated starting from the apex of the cone or pyramid.
- the shape of the recess portion 22 a is shown as that of a quadrangular pyramid, but the shape of the recess portion 22 a may be any one selected from conical or pyramidal shape, and may be a polygonal pyramid other than the quadrangular pyramid, or a circular cone.
- the depth of the recess portion 22 a is not particularly limited, and the upper limit thereof is the thickness of the negative electrode active material layer 22 .
- FIG. 2 is a view of the negative electrode active material layer 22 singly viewed from the electrolyte layer 4 side.
- the recess portions 22 a are regularly arranged as rectangular openings in a row-like shape, but the arrangement of the recess portions 22 a is not limited thereto.
- the openings of the recess portions 22 a may be alternately and regularly arranged, or may be irregularly arranged to some extent.
- the recess portions 22 a are preferably formed on the entire surface of the negative electrode active material layer 22 , the surface being adjacent to the electrolyte layer 4 .
- a planar portion 22 b is a face substantially perpendicular to the laminating direction of the negative electrode active material layer 22 .
- the planar portion 22 b is a portion where the recess portion 22 a is not formed on the surface of the negative electrode active material layer 22 , the surface being adjacent to the electrolyte layer 4 .
- the negative electrode active material layer 22 has the planar portion 22 b together with the recess portion 22 a , and thereby the negative electrode active material layer 22 can be formed without forming a projective portion capable of having a high current density in the negative electrode active material layer 22 closer to the electrolyte layer 4 . Therefore, formation of dendrites in a zone close to the electrolyte layer 4 can be suppressed. As shown in FIG.
- each of the planar portions 22 b is preferably disposed between the plurality of recess portions 22 a .
- the openings of the plurality of recess portions 22 a are not in close contact with each other.
- the positive electrode layer 30 is formed by forming a positive electrode active material layer 31 , for example, on a positive electrode current collector 32 .
- the positive electrode active material layer 31 is a layer containing a positive electrode active material as an essential component.
- the positive electrode active material layer 31 may contain a binder, a conductive auxiliary agent, an electrolyte, and the like.
- the binder, the conductive auxiliary agent, the electrolyte, and the like are not particularly limited, and known substances can be used as the electrode material of a secondary battery.
- the positive electrode active material is not particularly limited, and a well-known substance can be applied as the positive electrode active material of a secondary battery.
- the positive electrode active material include layered positive electrode active material particles such as LiCoO 2 , LiNiO 2 , LiCo 1/3 Ni 1/3 Mn 1/3 O 2 , LiVO 2 , LiCrO 2 , etc., spinel positive electrode active materials such as LiMn 2 O 4 , Li(Ni 0.25 Mn 0.75 ) 2 O 4 , LiCoMnO 4 , Li 2 NiMn 3 O 8 , etc., and olivine positive electrode active materials such as LiCoPO 4 , LiMnPO 4 , LiFePO 4 , etc.
- the positive electrode current collector 32 is not particularly limited, and a well-known substance can be applied as the positive electrode current collector of a secondary battery.
- Examples of the positive electrode current collector 32 include aluminum and stainless steel. Aluminum, stainless steel, or the like is molded into a foil shape, for example, and used. In addition to the above, a conductive carbon sheet (e.g., a graphite sheet or a CNT sheet) or the like may be used.
- the electrolyte layer 4 may be a layer containing a solid electrolyte or a layer containing an electrolytic solution in which the electrolyte is dissolved in a nonaqueous solvent.
- the electrolyte layer 4 is preferably a layer containing a solid electrolyte.
- the solid electrolyte contained in the electrolyte layer 4 a well-known substance as a solid electrolyte usable in a secondary battery can be applied.
- the solid electrolyte include a sulfide-based solid electrolyte, an oxide-based solid electrolyte, a nitride-based solid electrolyte, a halide-based solid electrolyte, etc.
- nonaqueous solvent-soluble electrolyte contained in the electrolyte layer 4 known substances can be applied as an electrolyte usable in a secondary battery.
- nonaqueous solvent for dissolving the liquid electrolyte examples include aprotic solvents such as carbonates, esters, ethers, nitriles, sulfones, lactones and the like.
- the battery cell 1 may include a separator.
- the separator is positioned between the positive electrode layer and the negative electrode layer.
- the material, thickness, and the like of the separator are not particularly limited, and a known separator such as polyethylene or polypropylene which can be used in a secondary battery cell can be applied.
- a known method of manufacturing a secondary battery can be employed except for the method of forming the negative electrode active material layer 22 having a recess portion and a planar portion on the surface of the negative electrode electrolyte layer, the surface being adjacent to the electrolyte layer.
- the negative electrode layer 20 and the positive electrode layer 30 may be formed by any method selected from a wet method and a dry method.
- a method in which an electrode material mixture slurry containing an electrode active material is applied to a current collector by a known method such as a doctor blade method and dried can be applied.
- a method of forming the negative electrode active material layer 22 having a recess portion and a planar portion for example, a method of pressing the negative electrode active material layer 22 formed on the negative electrode current collector 21 in the negative electrode layer 20 manufactured as described above, against a surface of a pressing device such as a uniaxial pressing device or a roll pressing device having irregularities formed thereon can be mentioned.
- the electrolyte layer 4 is a solid electrolyte layer having a solid electrolyte
- the electrolyte layer 4 can be formed through a step of pressing the solid electrolyte.
- the electrolyte layer 4 may be formed through a step of coating a surface of a substrate or an electrode with a solid electrolyte paste prepared by dispersing a solid electrolyte or the like in a solvent.
- the battery cell 1 is obtained by laminating the negative electrode layer 20 , the electrolyte layer 4 , and the positive electrode layer 30 in this order to form a laminate. At this time, a step of pressing the laminate may be performed.
- a means for pressing a known means such as a roll press can be used.
- Lithium metal serving as a negative electrode active material was bonded to a copper foil serving as a negative electrode current collector by a cladding material, and then pressing was performed using a uniaxial pressing device having irregularities on the surface thereof to prepare a negative electrode active material layer in which recess portions in the shape of quadrangular pyramid and planar portions were regularly arranged on the surface, as shown in FIG. 2 . Then, the solid electrolyte layer and the positive electrode layer manufactured by conventional methods and the negative electrode active material layer manufactured by the above method were laminated and integrally pressed to prepare a battery cell according to the Example.
- a battery cell according to the Comparative Example was manufactured in the same manner as in the Example except that no cone or pyramid-shaped recess portions were formed on the surface of the negative electrode active material layer.
- a cycle characteristic test (0.3 C, 60° C.) was performed using the battery cells of the Example and Comparative Example manufactured in the above. Charge and discharge of each of the battery cells of the Example and the Comparative Example was repeated 90 cycles and the relation between the number of cycles and the discharge capacity (mAh) is shown in FIG. 3 .
Abstract
To provide a battery cell capable of suppressing deposition of dendrites and improving cycle characteristics. A battery cell having a negative electrode layer, an electrolyte layer, and a positive electrode layer, the negative electrode layer comprising a negative electrode active material layer that has at least one recess portion and at least one planar portion on a surface of the negative electrode active material layer, the surface being adjacent to the electrolyte layer, the recess portion being a cone or pyramid-shaped recess portion having a slant portion. The negative electrode active material layer comprises lithium metal, and the electrolyte layer is preferably a solid electrolyte layer comprising a solid electrolyte. When the at least one recess portion and the at least one planar portion comprise a plurality of recess portions and a plurality of planar portions, respectively, each of the planar portions is formed between the plurality of recess portions.
Description
- This application is based on and claims the benefit of priority from Japanese Patent Application No. 2022-026392, filed on 24 Feb. 2022, the content of which is incorporated herein by reference.
- The present invention relates to battery cells.
- Conventionally, secondary batteries such as a lithium-ion secondary battery which have a high energy density have been widely used. In recent years, from viewpoints of improving energy efficiency, reducing negative impacts on the global environment by increasing the share of renewable energy and reducing CO2, the use of secondary batteries has been considered for various applications such as in-vehicle use. A secondary battery has a structure in which a solid electrolyte (separator) is provided between a positive electrode and a negative electrode and which is filled with a liquid or solid electrolyte (electrolytic solution).
- As a negative electrode active material of the secondary battery, metals such as lithium metal are used. However, when lithium metal is used as a negative electrode active material, there is a problem that short circuit occurs due to deposition of dendrites. In particular, in a solid battery having a solid electrolyte, the short circuit may occur when uneven distribution of restraining load occurs.
- As a lithium secondary battery negative electrode in which growth of dendrite crystals is suppressed, for example, a technique is known in which a large number of crystals are generated by forming a large number of crystal nuclei serving as crystal growth points in the negative electrode, whereby generation of large dendrite crystals is suppressed (see Patent Document 1).
- Patent Document 1: Japanese Unexamined Patent Application, Publication No. H6-84512
- The technique disclosed in Patent Document 1 is capable of suppressing generation of large dendrite crystals by forming fine irregularities on the substrate surface, but when the technique is applied to, for example, a solid-state battery, a strong restraining load is applied to the electrode, so that generation of even relatively small dendrite crystals may affect battery performance. Therefore, under the current state of development, satisfactory cycle characteristics during charge and discharge of the battery cell have not yet been obtained.
- The present invention has been made in view of the above-mentioned circumstances, and it is an object of the present invention to provide a battery cell capable of suppressing deposition of dendrites and improving cycle characteristics.
- A first aspect of the present invention relates to a battery cell having a negative electrode layer, an electrolyte layer, and a positive electrode layer, the negative electrode layer including a negative electrode active material layer that has at least one recess portion and at least one planar portion on a surface of the negative electrode active material layer, the surface being adjacent to the electrolyte layer, the recess portion being a cone or pyramid-shaped recess portion having a slant portion.
- According to the first aspect, a battery cell capable of suppressing deposition of dendrites and improving cycle characteristics can be provided.
- A second aspect of the present invention relates to the battery cell as described in the first aspect, in which the negative electrode active material layer contains lithium metal.
- According to the second aspect, even when lithium metal which easily produces dendrites is used as the negative electrode active material, occurrence of short circuit can be suppressed, and a battery cell having preferable cycle characteristics can be provided.
- A third aspect of the present invention relates to the battery cell as described in the first or second aspect, in which the electrolyte layer is a solid electrolyte layer including a solid electrolyte.
- According to the third aspect, even in a battery cell having a solid electrolyte layer containing a solid electrolyte as the electrolyte layer, occurrence of short circuit can be suppressed, and a battery cell having preferable cycle characteristics can be provided.
- A fourth aspect of the present invention relates to the battery cell as described in any one of the first to third aspects, in which the at least one recess portion and the at least one planar portion comprise a plurality of recess portions and a plurality of planar portions, respectively, and the plurality of planar portions are formed in a manner that the plurality of recess portions are not in contact with each other.
- According to the fourth aspect, even when a plurality of recess portions is formed in the negative electrode active material layer, no projective portions are formed on a surface of the negative electrode active material layer, the surface being adjacent to the electrolyte layer, and accordingly dendrites can be generated preferentially in the recess portions, which more preferably suppresses occurrence of short circuit of the battery cell.
-
FIG. 1 is a cross-sectional view illustrating a configuration of a battery cell according to an embodiment of the present invention; -
FIG. 2 is a top view illustrating a part of the negative electrode active material layer according to an embodiment of the present invention; and -
FIG. 3 is a graph illustrating results of cycle characteristic tests using the battery cells of the Example and the Comparative Example. - Hereinafter, a battery cell 1 according to an embodiment of the present invention will be described. As shown in
FIG. 1 , the battery cell 1 according to the present embodiment is formed by laminating anegative electrode layer 20, anelectrolyte layer 4, and apositive electrode layer 30 in this order. The battery cell 1 is, for example, a lithium-ion battery cell using lithium ions as a charge transfer medium. The battery cell 1 may be a battery cell having aliquid electrolyte layer 4. On the other hand, since the configuration of the present embodiment shown below can preferably reduce the influence of the deposition of dendrites, the battery cell 1 according to the present embodiment is preferably a battery cell having asolid electrolyte layer 4 which is susceptible to the influence of the deposition of dendrites. - The
negative electrode layer 20 is formed, for example, by forming a negative electrodeactive material layer 22 on a negative electrodecurrent collector 21. - The negative electrode
current collector 21 is not particularly limited, and a well-known substance can be applied as the negative electrode current collector of a solid secondary battery. Examples of the negative electrodecurrent collector 21 include copper, stainless steel, and the like. Copper, stainless steel, and the like are molded into, for example, a foil shape and used. - The negative electrode
active material layer 22 is a layer containing a negative electrode active material as an essential component. In addition to the negative electrode active material, the negative electrodeactive material layer 22 may contain a binder, a conductive auxiliary agent, an electrolyte, and the like. The binder, the conductive auxiliary agent, the electrolyte, and the like are not particularly limited, and known substances can be used as the electrode material for a secondary battery. - The negative electrode active material is not particularly limited, and a known substance can be applied as the negative electrode active material for the secondary batteries. On the other hand, the configuration of the present embodiment described below can preferably reduce the influence of deposition of dendrites, which is significant when lithium metal is used as the negative electrode active material. Accordingly, the negative electrode
active material layer 22 preferably contains lithium metal as the negative electrode active material. - Examples of the negative electrode active material other than lithium metal include lithium transition metal oxides such as lithium titanate (Li4Ti5O12); transition metal oxides such as TiO2, Nb2O3, WO3, etc.; metal sulfides; metal nitrides; carbon materials such as graphite, soft carbon, hard carbon, etc.; metal indium; lithium alloys; and the like.
- As shown in
FIGS. 1 and 2 , the negative electrodeactive material layer 22 has a plurality ofrecess portions 22 a and a plurality ofplanar portions 22 b on the surface of the negative electrodeactive material layer 22, the surface being adjacent to theelectrolyte layer 4. - As shown in
FIGS. 1 and 2 , arecess portion 22 a is a cone or pyramid-shaped recess portion having a slant portion S. Since therecess portions 22 a are formed in the negative electrodeactive material layer 22, the current density varies, and the current density increases in the vicinity of therecess portions 22 a. As a result, since dendrites are preferentially generated at therecess portion 22 a, the risk that the dendrites break through theelectrolyte layer 4 and short circuit occurs can be reduced. Thereby, the cycle characteristics of the battery cell 1 can be improved. In addition to the above, therecess portion 22 a can alleviate unevenness of pressure distribution caused by expansion of thenegative electrode layer 20 during charge of the battery cell 1. Further, since the contact area between theelectrolyte layer 4 and the negative electrodeactive material layer 22 is increased by therecess portion 22 a, resistance is reduced, and thus the output of the battery cell 1 is improved. - Since the
recess portion 22 a has a shape of cone or pyramid having a slant portion S, a dendrite is likely to be preferentially generated starting from the apex of the cone or pyramid. InFIGS. 1 and 2 , the shape of therecess portion 22 a is shown as that of a quadrangular pyramid, but the shape of therecess portion 22 a may be any one selected from conical or pyramidal shape, and may be a polygonal pyramid other than the quadrangular pyramid, or a circular cone. - The depth of the
recess portion 22 a is not particularly limited, and the upper limit thereof is the thickness of the negative electrodeactive material layer 22. -
FIG. 2 is a view of the negative electrodeactive material layer 22 singly viewed from theelectrolyte layer 4 side. InFIG. 2 , therecess portions 22 a are regularly arranged as rectangular openings in a row-like shape, but the arrangement of therecess portions 22 a is not limited thereto. The openings of therecess portions 22 a may be alternately and regularly arranged, or may be irregularly arranged to some extent. Therecess portions 22 a are preferably formed on the entire surface of the negative electrodeactive material layer 22, the surface being adjacent to theelectrolyte layer 4. - A
planar portion 22 b is a face substantially perpendicular to the laminating direction of the negative electrodeactive material layer 22. Theplanar portion 22 b is a portion where therecess portion 22 a is not formed on the surface of the negative electrodeactive material layer 22, the surface being adjacent to theelectrolyte layer 4. The negative electrodeactive material layer 22 has theplanar portion 22 b together with therecess portion 22 a, and thereby the negative electrodeactive material layer 22 can be formed without forming a projective portion capable of having a high current density in the negative electrodeactive material layer 22 closer to theelectrolyte layer 4. Therefore, formation of dendrites in a zone close to theelectrolyte layer 4 can be suppressed. As shown inFIG. 2 , each of theplanar portions 22 b is preferably disposed between the plurality ofrecess portions 22 a. In other words, it is preferable that the openings of the plurality ofrecess portions 22 a are not in close contact with each other. - The
positive electrode layer 30 is formed by forming a positive electrodeactive material layer 31, for example, on a positive electrodecurrent collector 32. - The positive electrode
active material layer 31 is a layer containing a positive electrode active material as an essential component. In addition to the positive electrode active material, the positive electrodeactive material layer 31 may contain a binder, a conductive auxiliary agent, an electrolyte, and the like. The binder, the conductive auxiliary agent, the electrolyte, and the like are not particularly limited, and known substances can be used as the electrode material of a secondary battery. - The positive electrode active material is not particularly limited, and a well-known substance can be applied as the positive electrode active material of a secondary battery. Examples of the positive electrode active material include layered positive electrode active material particles such as LiCoO2, LiNiO2, LiCo1/3Ni1/3Mn1/3O2, LiVO2, LiCrO2, etc., spinel positive electrode active materials such as LiMn2O4, Li(Ni0.25Mn0.75)2O4, LiCoMnO4, Li2NiMn3O8, etc., and olivine positive electrode active materials such as LiCoPO4, LiMnPO4, LiFePO4, etc.
- The positive electrode
current collector 32 is not particularly limited, and a well-known substance can be applied as the positive electrode current collector of a secondary battery. Examples of the positive electrodecurrent collector 32 include aluminum and stainless steel. Aluminum, stainless steel, or the like is molded into a foil shape, for example, and used. In addition to the above, a conductive carbon sheet (e.g., a graphite sheet or a CNT sheet) or the like may be used. - The
electrolyte layer 4 may be a layer containing a solid electrolyte or a layer containing an electrolytic solution in which the electrolyte is dissolved in a nonaqueous solvent. Theelectrolyte layer 4 is preferably a layer containing a solid electrolyte. - As the solid electrolyte contained in the
electrolyte layer 4, a well-known substance as a solid electrolyte usable in a secondary battery can be applied. Examples of the solid electrolyte include a sulfide-based solid electrolyte, an oxide-based solid electrolyte, a nitride-based solid electrolyte, a halide-based solid electrolyte, etc. - As a nonaqueous solvent-soluble electrolyte contained in the
electrolyte layer 4, known substances can be applied as an electrolyte usable in a secondary battery. - Examples of the nonaqueous solvent-soluble electrolyte include LiPF6, LiBF4, LiClO4, LiN(SO2CF3), LiN(SO2C2F5)2, LiCF3SO3, LiC4F9SO3, LiC(SO2CF3)3, LiF, LiCl, LiI, Li2S, Li3N, Li3P, Li10GeP2S12 (LGPS) , Li3PS4, Li6PS5Cl, Li7P2S8I, LixPOyNz (x=2y+3z−5, LiPON) , Li7La3Zr2O12 (LLZO) , Li3xLa2/3−xTiO3 (LLTO), Li1+xAlxTi2−x(PO4)3 (0≤x≤1, LATP), Li1.5Al0.5Ge1.5(PO4)3 (LAGP), Li1+x+yAlxTi2−xSiyP3−yO12, Li1+x+yAlx(Ti, Ge)2−xSiyP3−yO12, Li4−2xZnxGeO4 (LISICON), and the like. The above-mentioned electrolytes may be used alone, or in a combination of two or more types thereof.
- Examples of the nonaqueous solvent for dissolving the liquid electrolyte include aprotic solvents such as carbonates, esters, ethers, nitriles, sulfones, lactones and the like.
- When the
electrolyte layer 4 contains an electrolytic solution, the battery cell 1 may include a separator. The separator is positioned between the positive electrode layer and the negative electrode layer. The material, thickness, and the like of the separator are not particularly limited, and a known separator such as polyethylene or polypropylene which can be used in a secondary battery cell can be applied. - As the method of manufacturing the battery cell 1 according to the above-mentioned embodiment, a known method of manufacturing a secondary battery can be employed except for the method of forming the negative electrode
active material layer 22 having a recess portion and a planar portion on the surface of the negative electrode electrolyte layer, the surface being adjacent to the electrolyte layer. - The
negative electrode layer 20 and thepositive electrode layer 30 may be formed by any method selected from a wet method and a dry method. For example, when thenegative electrode layer 20 and thepositive electrode layer 30 are formed by the wet method, a method in which an electrode material mixture slurry containing an electrode active material is applied to a current collector by a known method such as a doctor blade method and dried can be applied. - As a method of forming the negative electrode
active material layer 22 having a recess portion and a planar portion, for example, a method of pressing the negative electrodeactive material layer 22 formed on the negative electrodecurrent collector 21 in thenegative electrode layer 20 manufactured as described above, against a surface of a pressing device such as a uniaxial pressing device or a roll pressing device having irregularities formed thereon can be mentioned. - When the
electrolyte layer 4 is a solid electrolyte layer having a solid electrolyte, theelectrolyte layer 4 can be formed through a step of pressing the solid electrolyte. Alternatively, theelectrolyte layer 4 may be formed through a step of coating a surface of a substrate or an electrode with a solid electrolyte paste prepared by dispersing a solid electrolyte or the like in a solvent. - The battery cell 1 is obtained by laminating the
negative electrode layer 20, theelectrolyte layer 4, and thepositive electrode layer 30 in this order to form a laminate. At this time, a step of pressing the laminate may be performed. As a means for pressing, a known means such as a roll press can be used. - The preferred embodiments of the present invention have been described above. The present invention is not limited to the description of the above embodiment, and can be appropriately modified without departing from the gist of the present invention.
- Hereinafter, the present invention will be described in more detail based on the Examples and the like, but the present invention is not limited to these Examples and the like.
- Lithium metal serving as a negative electrode active material was bonded to a copper foil serving as a negative electrode current collector by a cladding material, and then pressing was performed using a uniaxial pressing device having irregularities on the surface thereof to prepare a negative electrode active material layer in which recess portions in the shape of quadrangular pyramid and planar portions were regularly arranged on the surface, as shown in
FIG. 2 . Then, the solid electrolyte layer and the positive electrode layer manufactured by conventional methods and the negative electrode active material layer manufactured by the above method were laminated and integrally pressed to prepare a battery cell according to the Example. - A battery cell according to the Comparative Example was manufactured in the same manner as in the Example except that no cone or pyramid-shaped recess portions were formed on the surface of the negative electrode active material layer.
- By using the battery cells of the Example and Comparative Example manufactured as described above, initial charge/discharge efficiency (0.1 C, 25° C.) and initial direct current resistance (DCR) (60° C.) were measured, but no significant difference was observed.
- A cycle characteristic test (0.3 C, 60° C.) was performed using the battery cells of the Example and Comparative Example manufactured in the above. Charge and discharge of each of the battery cells of the Example and the Comparative Example was repeated 90 cycles and the relation between the number of cycles and the discharge capacity (mAh) is shown in
FIG. 3 . In the Comparative Example, the cycle characteristics were tested at N=2. As shown inFIG. 3 , when compared with the battery cell of the Comparative Example, the discharge capacity of the battery cell of the Example hardly decreased even when the number of cycles was increased, and the result of excellent cycle characteristics is apparent. - 1 Battery cell
- 20 Negative electrode layer
- 22 Negative electrode active material layer
- 22 a Recess portion
- 22 b Planar portion
- 30 Positive electrode layer
- 4 Electrolyte layer
- S Slant portion
Claims (4)
1. A battery cell having a negative electrode layer, an electrolyte layer, and a positive electrode layer,
the negative electrode layer comprising a negative electrode active material layer that has at least one recess portion and at least one planar portion on a surface of the negative electrode active material layer, the surface being adjacent to the electrolyte layer,
the recess portion being a cone or pyramid-shaped recess portion having a slant portion.
2. The battery cell according to claim 1 , wherein the negative electrode active material layer comprises lithium metal.
3. The battery cell according to claim 1 , wherein the electrolyte layer is a solid electrolyte layer comprising a solid electrolyte.
4. The battery cell according to claim 1 , wherein the at least one recess portion and the at least one planar portion comprise a plurality of recess portions and a plurality of planar portions, respectively and each of the planar portions is formed between the plurality of recess portions.
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JP2022-026392 | 2022-02-24 |
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